期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 10, 期 11, 页码 3777-3786出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.2c00800
关键词
heterogeneous catalysis; reductive amination; amines; imines; switchable selectivity
In this study, a facile strategy was developed to synthesize two carbon-doped Ni catalysts, which can switch the selectivity in the reductive amination of biomass-derived carbonyl compounds and exhibit excellent stability and a broad substrate scope.
Reductive aminations of biomass-derived carbonyl compounds, an industrially important class of reactions applied for green and sustainable production of valuable amines/imines, often suffer from problems of selectivity toward the target product and reusability of the catalyst. Herein, we develop a facile strategy to synthesize two carbon-doped Ni catalysts with particle sizes of 7.5 and 47.5 nm, respectively, over which the selectivity in the reductive amination of biomass-derived carbonyl compounds is completely switched between primary amines (>96% yield, 7.5 nm) and secondary imines (>97% yield, 47.5 nm). The synthesis is derived from the confined pyrolysis of Ni-Al layered double hydroxides (NiAl-LDH) grafted on hollow polymer nanospheres (HPS), in which the HPS play four roles (i.e., template, reductant, carbon resource, and Ni size controller). The two catalysts exhibit excellent stability due to the existence of surface Ni-C-x species. Reductive aminations over these two catalysts have a broad substrate scope and can be scaled up to the gram level, indicating the potential for industrial applications.
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